Fe3Se4/FeSe heterojunctions in cornstalk-derived N-doped carbon framework enhance charge transfer and cathodic oxygen reduction reaction to boost bio-electricity generation
Fe3Se4/FeSe heterojunctions in cornstalk-derived N-doped carbon framework enhance charge transfer and cathodic oxygen reduction reaction to boost bio-electricity generation
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玉米杆衍生的氮掺杂碳骨架中的 Fe3Se4/FeSe 异质结增强电荷转移和阴极氧还原反应，从而促进生物发电
DOI：
10.1016/j.apcatb.2018.11.074
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发表时间：
2019-05
期刊：
影响因子：
--
通讯作者：
Zou Jinlong
中科院分区：
文献类型：
--
作者：
Jing Baojian;You Shijie;Ma Yuanyuan;Xing Zipeng;Chen Hun;Dai Ying;Zhang Chunyue;Ren Nanqi;Zou Jinlong
微生物燃料电池（ac - mfc）空气阴极氧还原反应（ORR）动力学迟缓是能量损失的主要障碍之一。本研究以废生物质（玉米秆芯）为原料，制备了氮掺杂Fe3Se4/FeSe/部分石墨化碳（Fe3Se4/FeSe/NPGC）复合材料作为非贵金属空气阴极（ORR）催化剂。随着碳化温度的升高（800 ~ 950℃），Fe3Se4与FeSe之间的晶相转变增强，形成Fe3Se4/FeSe异质结。在ac - mfc中，Fe3Se4/FeSe/NPGC（850°C）阴极获得了最高的功率密度（1003 mW m−2）和耐久性（运行105 d后下降7.8%），高于Pt/C （840 mW m−2,52.4%）。Fe3Se4/FeSe/NPGC（850℃）具有较高的ORR活性，部分原因是其比表面积大（356.68 m2 - 1）和多孔结构。碳骨架中掺杂的N原子（吡啶N、吡啶N和石墨N）增强了C原子的电荷离域，减少了电子损失，通过四电子（4e−）ORR途径提高了电子利用率。Fe3Se4/FeSe异质结将大大提高电荷转移和氧解离效率。高导电性的NPGC骨架也有助于有效的电荷转移。采用Fe3Se4/FeSe/NPGC（850°C）阴极的ac - mfc具有良好的长期耐久性，主要是由于其ORR动力学快，仍能生成少量（低于10.0%）H2O2（•OH和•O2−）中间体，抑制阴极表面电生微生物的生长。这项工作不仅为ORR的碳负载过渡金属硒化物提供了基础研究，而且为交流- mfc的贵金属基电极提供了一种新的有前途的替代品。
Sluggish kinetics of oxygen reduction reaction (ORR) on air-cathode of microbial fuel cells (AC-MFCs) is one of the main obstacles for energy loss. In this study, nitrogen-doped Fe3Se4/FeSe/partially-graphitized carbon (Fe3Se4/FeSe/NPGC) composites as non-precious-metal air-cathode (ORR) catalysts are obtained using waste biomass (cornstalk cores) as raw material. As carbonization temperature increases (800–950 °C), the crystalline phase transition between Fe3Se4and FeSe is strengthened to form the Fe3Se4/FeSe heterojunctions. The highest power density (1003 mW m−2) and durability (decline of 7.8% after 105 d operation) are obtained by Fe3Se4/FeSe/NPGC (850 °C) cathode in AC-MFCs, which are higher than those of Pt/C (840 mW m−2, 52.4%). The high ORR activity of Fe3Se4/FeSe/NPGC (850 °C) is partly attributed to the large specific surface area (356.68 m2g−1) and porous structure. Doped N atoms (pyridinic N, pyrrolic N and graphitic N) in carbon skeleton enhance the charge delocalization of C atoms to reduce the electron loss to enhance the electron utilization via a four-electron (4e−) ORR pathway. Fe3Se4/FeSe heterojunctions should greatly promote the charge transfer and oxygen dissociation efficiencies. The highly-conductive NPGC skeleton also contributes to the efficient charge transfer. The good long-term durability of AC-MFCs with Fe3Se4/FeSe/NPGC (850 °C) cathode is mainly ascribed to its fast ORR kinetics, which still generates a small amount (below 10.0%) of H2O2(•OH and •O2−) intermediate to inhibit the electrogenic microbe growth on cathode surface. This work not only provides the fundamental studies on carbon-supported transition-metal selenides for ORR, but also provides a new kind of promising alternatives for precious metal-based electrodes for AC-MFCs.
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